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Unusual Li2O sublimation promotes single-crystal growth and sintering

Author

Listed:
  • Bingbin Wu

    (Pacific Northwest National Laboratory)

  • Ran Yi

    (Pacific Northwest National Laboratory)

  • Yaobin Xu

    (Pacific Northwest National Laboratory)

  • Peiyuan Gao

    (Pacific Northwest National Laboratory)

  • Yujing Bi

    (Pacific Northwest National Laboratory)

  • Libor Novák

    (Thermo Fisher Scientific)

  • Zhao Liu

    (Thermo Fisher Scientific)

  • Enyuan Hu

    (Brookhaven National Laboratory)

  • Nan Wang

    (Brookhaven National Laboratory)

  • Job Rijssenbeek

    (Albemarle Corporation)

  • Subramanian Venkatachalam

    (Albemarle Corporation)

  • Jing Wu

    (Pacific Northwest National Laboratory)

  • Dianying Liu

    (Pacific Northwest National Laboratory)

  • Xia Cao

    (Pacific Northwest National Laboratory)

  • Jie Xiao

    (Pacific Northwest National Laboratory
    University of Washington)

Abstract

Li2O is rarely used for cathode material synthesis due to its high melting point (1,438 °C). Here we discover that Li2O can sublimate at 800–1,000 °C under ambient pressure, opening new possibilities for cathode synthesis. We propose a mechanism that enables synthesis of single crystals—such as LiNi0.8Mn0.1Co0.1O2 (NMC811) or LiNi0.9Mn0.05Co0.05O2 (NMC90)—without direct contact with Li2O salts. We show that Li2O vapour successfully converts spent polycrystalline NMC811 into segregated single crystals without milling or post-treatment. The Li2O vapour, derived from Li2O solids, diffuses rapidly and reacts with precursors, mimicking a molten-salt environment, which facilitates single-crystal growth. The chemical lithiation process continuously drives Li2O sublimation, sintering the crystals. Single crystals derived from Li2O and fresh precursors or spent polycrystals exhibit outstanding cycling after 1,000 cycles in full cells. The demonstrated Li2O sublimation and its universal role in promoting single-crystal growth provides an effective approach for single-crystal synthesis, scale-up and recycling.

Suggested Citation

  • Bingbin Wu & Ran Yi & Yaobin Xu & Peiyuan Gao & Yujing Bi & Libor Novák & Zhao Liu & Enyuan Hu & Nan Wang & Job Rijssenbeek & Subramanian Venkatachalam & Jing Wu & Dianying Liu & Xia Cao & Jie Xiao, 2025. "Unusual Li2O sublimation promotes single-crystal growth and sintering," Nature Energy, Nature, vol. 10(5), pages 605-615, May.
    • Handle: RePEc:nat:natene:v:10:y:2025:i:5:d:10.1038_s41560-025-01738-4
    DOI: 10.1038/s41560-025-01738-4
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    References listed on IDEAS

    as
    1. Jie Xiao & Nicole Adelstein & Yujing Bi & Wenjuan Bian & Jordi Cabana & Corie L. Cobb & Yi Cui & Shen J. Dillon & Marca M. Doeff & Saiful M. Islam & Kevin Leung & Mengya Li & Feng Lin & Jun Liu & Hong, 2024. "Assessing cathode–electrolyte interphases in batteries," Nature Energy, Nature, vol. 9(12), pages 1463-1473, December.
    2. Un-Hyuck Kim & Geon-Tae Park & Byoung-Ki Son & Gyeong Won Nam & Jun Liu & Liang-Yin Kuo & Payam Kaghazchi & Chong S. Yoon & Yang-Kook Sun, 2020. "Heuristic solution for achieving long-term cycle stability for Ni-rich layered cathodes at full depth of discharge," Nature Energy, Nature, vol. 5(11), pages 860-869, November.
    3. Moonsu Yoon & Yanhao Dong & Yimeng Huang & Baoming Wang & Junghwa Kim & Jin-Sung Park & Jaeseong Hwang & Jaehyun Park & Seok Ju Kang & Jaephil Cho & Ju Li, 2023. "Eutectic salt-assisted planetary centrifugal deagglomeration for single-crystalline cathode synthesis," Nature Energy, Nature, vol. 8(5), pages 482-491, May.
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